To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals with minimal carbon emissions. The background of such N-cycles, such as nitrogen fixation, ammonia oxidation, and nitrate reduction, is briefly introduced here. The discussion of emerging nanostructures in various conversion reactions is focused on the architecture/compositional design, electrochemical performances, reaction mechanisms, and instructive tests. Energy device advancements for achieving more functions as well as in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed reactions as well as less discussed C–N coupling reactions are also summarized. We classify inorganic nitrogen sources that convert to each other under an applied voltage into three types, namely, abundant nitrogen, toxic nitrate (nitrite), and nitrogen oxides, and useful compounds such as ammonia, hydrazine, and hydroxylamine, with the goal of providing more critical insights into strategies to facilitate the development of our circular nitrogen economy.

https://www.sciopen.com/article_pdf/1531201054523838466.pdf

Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Two-dimensional (2D) transition metal oxide and chalcogenide (TMO&C)-based photocatalysts have recently attracted significant attention for addressing the current worldwide challenges of energy shortage and environmental pollution. The ultrahigh surface area and unconventional physiochemical, electronic and optical properties of 2D TMO&Cs have been demonstrated to facilitate photocatalytic applications. This review provides a concise overview of properties, synthesis methods and applications of 2D TMO&C-based photocatalysts. Particular attention is paid on the emerging strategies to improve the abilities of light harvesting and photoinduced charge separation for enhancing photocatalytic performances, which include elemental doping, surface functionalization as well as heterojunctions with semiconducting and conductive materials. The future opportunities regarding the research pathways of 2D TMO&C-based photocatalysts are also presented.

/pdf/two-dimensional-transition-metal-oxide-and-chalcogenide-5437ubn9zd.pdf

Two-Dimensional Transition Metal Oxide and Chalcogenide-Based Photocatalysts

This paper describes synthesis and characterization of Ni and Ni-Co alloy supported over SiO 2 derived from phyllosilicates. A series of 10 wt% Ni-Co phyllosilicate supported over SiO 2 with different Ni/Co ratio is successfully prepared by hydrothermal method where urea is used to release ammonia gradually providing a basic environment. TPR results show that adding of Co enhances the metal-support interaction. After H 2 reduction at high temperature, small and uniform Ni-Co alloy particles are well supported over silica. These catalysts are tested for dry reforming of methane (DRM) at 750 °C. The catalytic performance is highly affected by Ni/Co ratio: 10Ni and 7Ni3Co show high and stable activity for 100 h, whereas 5Ni5Co, 3Ni7Co and 10Co exhibit severe deactivation due to oxidation of metal sites. A harsher test has shown that adding of Co with a proper amount indeed can help to suppress metal sintering and carbon formation.

Highly carbon-resistant Ni–Co/SiO2 catalysts derived from phyllosilicates for dry reforming of methane

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase of nitrate level in surface and ground waters, and substantial emission of nitrogen oxides causes heavy air pollution. Nitrogen gas, as the main component of air, has been used for mass ammonia production for over a century, providing enough nutrition for agriculture to support world population increase. In the last decade, researchers have made great efforts to develop ammonia processes under ambient conditions to combat the intensive energy consumption and high carbon emission associated with the Haber-Bosch process. Among different techniques, electrochemical nitrate reduction reaction (NO3 RR) can achieve nitrate removal and ammonia generation simultaneously using renewable electricity as the power, and there is an exponential growth of studies in this research direction. Here we provide a timely and comprehensive review on the important progresses of electrochemical NO3 RR, covering the rational design of electrocatalysts, emerging C-N coupling reactions, and advanced energy conversion and storage systems. Moreover, future perspectives are proposed to accelerate the industrialized NH3 production and green synthesis of chemicals, leading to a sustainable nitrogen cycle via prosperous N-based electrochemistry. This article is protected by copyright. All rights reserved.

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond.

Enhanced stability of Ni/SiO2 catalyst for CO2 methanation: Derived from nickel phyllosilicate with strong metal-support interactions

Ammonia-assisted synthesis towards a phyllosilicate-derived highly-dispersed and long-lived Ni/SiO2 catalyst

Electro-reduction of nitrate to ammonia (e-NRA) has been considered as a facile and promising approach to eliminate nitrate pollution and produce ammonia (NH3) under ambient conditions. Nevertheless, in recent state-of-the-art...

In-Situ Reconstruction Enhanced Dual-Site Catalysis towards Nitrate Electroreduction to Ammonia

Vanadium phosphorus oxide (VPO) catalysts supported on CeO 2 and P-modified CeO 2 (P-CeO 2 ) have been firstly synthesized for selective oxidation of n -butane to maleic anhydride (MA). The catalysts supported on P-CeO 2 showed higher catalytic performance, especially higher MA selectivity than catalysts on pure ceria, and their specific activities (normalized to per unit mass of VPO loading) were also superior to that of bulk VPO. TG, TEM, XRD, Raman, H 2 -TPR and XPS results revealed that the structure and property of VPO are largely affected by the support. The loaded VPO existed almost wholly as VOPO 4 phases on pure ceria, while mainly in the form of (VO) 2 P 2 O 7 with small amount of VOPO 4 phases on phosphorus-modified ceria. Both VPO/P-CeO 2 and bulk VPO catalysts have the similar VPO phase structure, but the former showed the enhanced reducibility of V 4+ phase. These differences in structure and properties of the catalysts were discussed and related to their different catalytic performances.

Enhancing catalytic performance of phosphorus-modified ceria supported VPO catalysts for n-butane oxidation

Facile preparation of porous flower-like ZnO microspheres with excellent photocatalytic performance

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Ammonia-assisted synthesis towards a phyllosilicate-derived highly-dispersed and long-lived Ni/SiO2 catalyst

In-Situ Reconstruction Enhanced Dual-Site Catalysis towards Nitrate Electroreduction to Ammonia

Enhancing catalytic performance of phosphorus-modified ceria supported VPO catalysts for n-butane oxidation

Facile preparation of porous flower-like ZnO microspheres with excellent photocatalytic performance